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Archives Massachusettsinstitute of Techmfllogy A COMPUTER MODEL OF THE RECTISOL PROCESS USING THE ASPEN SIMULATOR by Rosalyn A. preston SUBMITTED IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF MASTER OF SCIENCE IN CHEMICAL ENGINEERING at the MASSACHUSETTS INSTITUTE OF TECHNOLOGY December, 1981 Q Massachusetts Institute of Technology 1981 Signature of Author Signatureof Author Department of Chemical Engineering December 7, 1981 Certified by Lawrence B. Evans Thesis Supervisor Accepted by Glenn C Williams Chairman, Departmental Graduate Committee Archives MASSACHUSETTSINSTiTUTE OF TECHMflLOGY JUN 1 13982 i IRRA!ES A COMPUTER MODEL OF THE RECTISOL PROCESS USING THE ASPEN SIMULATOR by Rosalyn A. Preston Submitted to the Department of Chemical Engineering on December 7, 1981 in partial fulfillment of the requirements for the Degree of Master of Science in Chemical Engineering ABSTRACT A computer model of the Rectisol process for acid gas absorption has been developed with the ASPEN process simulator. The model uses a modified ver- sion of the Redlich-Kwong-Soave equation-of-state to represent the phase equilibria for the methanol- water-aromatics-acid gas system. This report de- scribes the development of the physical properties model and the flowsheet simulation. The work is based on the CONOCO design for a commercial scale coal gasification facility. The computer modelling effort was carried out under contract to the Morgan- town Energy Technical Center, U. S. Department of Energy. TABLE OF CONTENTS ACKNOWLEDGEMENTS .... ....... ... vii I. INTRODUCTION . ...... ....... .. .. II. AC:ID GAS ABSORPTION PROCESSES ...... .6 General Features of Acid Gas Absorption . a . 6 Processes . .... ... .... ... · · · 6 Absorption ........ ..... a1 a a 7 Regeneration . .. ... .. a a a 7 Solvent Selection . ....... * a a 9 Heat Integration .... ...... * a a 10 Solvent Recovery ........a . .. 12 Advantages of the Rectisol Process ... a a 12 Rectisol Process Description . ..... * a a 13 III. DEVELOPMENT OF PHYSICAL PROPERTIES MODEL .. a a 19 Selection of the Thermodynamic Model .. a .. 19 Modified Redlich-Kwong-SoaveEquation-of-State 21 Experimental Phase Equilibrium Data .... 23 Development of Modified Redlich-Kwong-Soave Model Parameters .... ...... ..... 25 Evaluation of the Preliminary Thermodynamic Model . ..... ........... 27 Enthalpy Calculations .. ...... ... 32 IV. SIMULATION OF THE RECTISOL PROCESS ..... ... 36 Basis for the Process Simulation . ...... 36 Absorption Section ..... ...... 38 Flash Regeneration Section .. ...... 43 Naphtha Extractor .... .... .. 43 Azeotrope Column ..... ..a a .a 44 Methanol-Water Column . ....... 49 iii Hot Regeneration Column .. * O . .. · 50 Water Wash Column ... a 0 0 · a a a 52 Heat Exchangers .... .. 52 Methanol Make-up . .... 53 a * a a a a a e· Flowsheet Convergence . ··· · 53 V. RECTISOL PROCESS SIMULATION RESULTS.... 55 VI.CONCLUSION. ........ ...U a a a a a a 59 APPENDIX A OVERALL RECTISOL MODEL APPENDIX B ABSORPTION SECTION SIM[LATION APPENDIX C AZEOTROPE COLUMN SIMUIL MTION APPENDIX D METHANOL-WATER COLUMN SIMULATION APPENDIX E HOT REGENERATION COLUMI[ SIMULATION APPENDIX F WATER WASH COLUMN SIMU LATION LITERATURE CITED BIBLI OGRAPHY iv LIST OF FIGURES 1. The Pipeline Gas Demonstration Plant . 2 2. The Rectisol Process . 4 3. Comparison of Equilibrium Loading of Chemical and Physical Solvents . .. 11 4. Block Flow Diagram of the Rectisol Process . 14 5. Process Flow Diagram of the Rectisol Process . 15 6. Process Flow Diagram of the Rectisol Process . 16 7. Henry's Law Constants for Nitrogen in a Methanol and Carbon Dioxide Mixture . 30 8. Block Flow Diagram of the Rectisol Computer Model 39 9. Effect of Solvent Rate and Number of Trays on Carbon Dioxide Absorption . ....... 42 10. Ternary Diagram for Methanol-Benzene-Water . 45 11. McCabe-Thiele Plot for Azeotrope Column . 48 v LIST OF TABLES 1. Comparison of Modified RKS Model Predictions with Experimental Data for Methanol-Hydrogen Sulfide- Carbon Dioxide- Nitrogen . 33 2. Binary Interaction Parameters for the Modified Redlich-Kwong-Soave Equation-of-State 34 ......... 3. Composition of Feed Gas to Rectisol Process 37 4. Desulfurized Gas Composition . .. 56 5. Acid Gas Composition . o. ..... .. 56 6. Regenerated Methanol Composition.. ........ 56 7. Cooling and Heating Duties for the Rectisol Process 58 vi ACKNOWLEDGMENTS I would like to express my appreciation to all the ASPEN staff who gave me help and support on this project, especially to Herb Britt and Chau-Chyun Chen for assisting me in almost every aspect, to Joe Boston and Paul Mathias for their help with modelling the physical properties, and to Willie Chan and Fred Ziegler for their debugging efforts. I would also like to thank my advisor, Professor L. B. Evans, forhis gui- dance and optimism throughout. vii I. INTRODUCTION The objective of this work was to develop a computer model of the Rectisol process (Hochgesand, 1970; Scholz, 1969) using the ASPEN process simulator. This simulation was pre- pared as part of a program to transfer ASPEN technology to the Morgantown Energy Technology Center (METC) of the United States Department of Energy. The overall program involved develop- ment of computer models for the major process units in the CONOCO Slagging Lurgi Coal Gasification process. The computer modelling effort took CONOCO's design for a commercial scale coal gasification facility as the basis (CONOCO, 1980). This facility, shown schematically in Figure 1, is designed to generate pipeline quality substitute natural gas from coal. Briefly, the process gasifies coal with steam and oxygen, generated by cryogenic air separation. The gas- ification takes place at high pressure in a moving bed slagging gasifier using Lurgi technology. Crude synthesis gas is re- covered from the top of the gasifier, while the ash is with- drawn in a molten slag form from the bottom. The synthesis gas is subsequently directed to the Rectisol unit for purifi- cation. Here, light oils and sulfur compounds are removed from the gas and recovered. Following purification, the gases are allowed to undergo water-gas shift and methanation reac- tions simultaneously. Carbon dioxide produced in the shift reaction must then be washed out with hot carbonate solution to improve the BTU quality of the substitute natural gas. The final gas treatment involves compression and drying. 1 w 2 cl Cd 0 Cd ro ad4 ordH a) c-) d E a) 3d for 0 E o0 EC E Cd o 0 a, - P .Ha) Ct= - W o 0 p xEC Cd 0 0\ TO 0co 0:z; e, 0oa) CD a, a) a) fAt o o 3 The Rectisol process itself features refrigerated meth- anol as the solvent into which the acid gases in the synthesis gas are absorbed. The process is comprised of an absorption section followed by a series of regeneration processes in which the rich solvent is purified and the absorbed compounds recov- ered. The diagram in Figure 2 illustrates the particular Rectisol design proposed for the CONOCO coal gasification facility. The Rectisol computer model described in this report provides a stream-by-stream heat and material balance for the process. In addition, the model predicts the composition of the outlet streams for a given set of operating conditions. Therefore, the model can be used to assess the effect of var- ious process variables on the composition of the desulfurized gas and acid gas products. The model also predicts the purity of the regenerated methanol solvent for specific regeneration operating conditions. Separate models of the absorbers and distillation columns yield a rigorous tray-to-tray analysis of each column. Overall, the Rectisol simulation represents a flexible tool which may be applied in future design and sen- sitivity studies and in trouble-shooting after process start- up. The input to the simulation is based on the process flow- sheet and feed streams from the CONOCO commercial design. Since Rectisol is a proprietary process licensed by Lurgi Min- eraloltechnik GmbH, the CONOCO design did not provide any in- formation on the actual process operating conditions. For this reason, development of the computer model entailed a 4 o .H 34 d i a) Z ) 0 ~o D ts o oo M *H O 0 Fz ¢ C: E0 U2 U) W o0 0 Ho a) U2a4 o &4 PE-4 .H 0 V: m X E E-1 Z 0 5 fair amount of design work to establish reasonable process operating conditions. The following chapters describe the development of the Rectisol model. The work initially involved a literature search to locate published process data regarding Rectisol. Subsequently, considerable effort was devoted to developing a good thermodynamic model of the system to provide adequate physical properties predictions. The actual computer model- ling work required testing of several ASPEN models which were still in the development stage. Further, it was necessary to perform sensitivity studies on the design variables in order to establish suitable operating conditions. It was orig- inally intended to use the final Rectisol model to examine the sensitivity of the process to various design variables. However, lack of computer funds curtailed the project once the model was developed. 6 II. ACID GAS ABSORPTION PROCESSES This section discusses the general features of acid gas absorption processes in order to provide some background for the detailed description of the Rectisol process. In addition, the discussion serves to present the basic design variables which must be considered in designing a process to remove acid gases. General Features of Acid Gas Absorption Processes Removal of acid gases, primarily carbon dioxide and hydro- gen sulfide, is important for many industrial plants producing a gaseous intermediate or final product. In the production of substitute natural gas by coal gasification, hydrogen is generated together with a substantial quantity of carbon dioxide. Since carbon dioxide has no heating value, it must be separated out of the final pipeline gas to raise the overall BTU value. The separation may occur at several points in the process. Removal prior to shift conversion of the carbon monoxide and water to hydrogen and carbon dioxide favors the equilibrium hydrogen concentration. However, since carbon dioxide is pro- duced in this reaction, further treating to remove carbon di- oxide may be required.
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